Journal Article

PreJuSER-20714

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Site-selective time resolved laser fluorescence spectroscopy of Eu and Cm dopted LaPO4

Holliday, K. S. ; Babelot, C.FZJ* ; Walther, C. ; Neumeier, S.FZJ* ; Bosbach, D.FZJ* ; Stumpf, T.

2012
Oldenbourg München

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Please use a persistent id in citations: http://hdl.handle.net/2128/18324  doi:10.1524/ract.2012.1900

Abstract: Samples of LaPO4 doped with Eu3+ or Cm3+ were synthesized by a hydrothermal process which resulted in a solid solution at temperatures less than conventional processing. Time resolved laser fluorescence spectroscopy was used to probe the incorporated Eu3+ or Cm3+ in order to gain structural information on its local environment. This revealed that Eu3+ and Cm3+ incorporate on the La site as expected. The emission spectrum of Eu3+ resolves the fully degenerate 5-fold splitting of the peaks in the F-2 transition due to the low symmetry of the site, confirming previous calculations. A minor site in the Eu3+ doped sample is identified as coordinated with hydroxide contamination. Direct excitation of Cm3+ doped samples show the presence of "satellite" species. Although these spectral features have been observed in Cm3+ doped LuPO4 and YPO4, this is the first time that these satellites are resolved into their individual species. These are hypothesized to be due to a disturbance in the ideal structure which creates a break in the equivalence of the four lanthanum sites within a unit cell. The 4-fold ground state splitting of all species is identical, although slightly shifted, indicating similar environments. The fluorescence lifetimes were long (1.2 ms for Cm and 3.6 ms for Eu) indicating an absence of water in the immediate coordination sphere due to the incorporation of the doping ion.

Keyword(s): J ; Lanthanum phosphate (auto) ; TRLFS (auto) ; Europium (auto) ; Site-selective (auto) ; Curium (auto)

Note: The authors thank Sebastian Buchner for technical assistance with TRLFS measurements. This work co-financed by the Helmholtz Gemeinschaft Deutscher Forschungszentren (HGF) by supporting the Helmholtz-Hochschul-Nachwuchsgruppe "Aufklarung geochemischer Reaktionsmechanismen an der Wasser/Mineralphasen Grenzflache". This work also was supported by the Ministerium fur Innovation, Wissenschaft, Forschung und Technologie (MIWFT) des Landes Nordrhein-Westfalen; AZ: 323-005-0911-0129.

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Contributing Institute(s):

1. Sicherheitsforschung und Reaktortechnik (IEK-6)

Research Program(s):

1. Nukleare Sicherheitsforschung (P14)

Appears in the scientific report 2012

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Database coverage:
; JCR ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection ; Zoological Record

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